solid state luminescent radiation imaging detectors...

34
Rosa Maria Montereali ENEA, C.R. Frascati, Technical Unit for the Development and Applications of Radiations, Photonics Micro- and Nano-structures Lab., Via E. Fermi 45, 00044 Frascati (Rome) Italy [email protected] , http://www.frascati.enea.it/UTAPRAD/lab_mnf.htm , http://www.enea.it/it/Ricerca_sviluppo/nuove-tecnologie 1 Solid state luminescent radiation imaging detectors based on LiF crystals and thin films 2 mm Proton beam image on a LiF film E = 3 MeV Soft X - ray radiography of a dragonfly wing on a LiF film E = 300 800 eV F. Bonfigli S. Libera M. Piccinini M.A.Vincenti ENEA C.R. Frascati E. Nichelatti ENEA C.R. Casaccia Phd of Industrial Engineering Research activities on Advanced Materials 8 Giugno 2015, Universita’ di Tor Vergata

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Rosa Maria MonterealiENEA, C.R. Frascati, Technical Unit for the Development and Applications of Radiations,

Photonics Micro- and Nano-structures Lab., Via E. Fermi 45, 00044 Frascati (Rome) Italy

[email protected],

http://www.frascati.enea.it/UTAPRAD/lab_mnf.htm, http://www.enea.it/it/Ricerca_sviluppo/nuove-tecnologie

1

Solid state luminescent radiation imaging detectors

based on LiF crystals and thin films

2 mmProton beam image on a LiF film

E = 3 MeV

Soft X-ray radiography of a dragonfly wing on a LiF film

E = 300 – 800 eV

F. Bonfigli

S. Libera

M. Piccinini

M.A.Vincenti

ENEA C.R.

Frascati

E. Nichelatti

ENEA C.R.

Casaccia

Phd of Industrial Engineering

Research activities on Advanced Materials

8 Giugno 2015, Universita’ di Tor Vergata

ENEA Italian National Agency for New Technologies,

Energy and Sustainable Economic Development

2

Main activities

•Research and experimentation on controlled nuclear

fusion, both magnetically confined and inertial;

•Development of specific technologies based on this

research, including superconductivity, neutron-matter

interaction, materials and automated maintenance;

•Research and development of laser sources (gas,

solid-state, free-electron) and of laser applications in

environmental, industrial and medical diagnostics,

nano and micro systems, metrology and laser vision;

•Research and development of electron and proton

accelerators for scientific, medical and industrial

applications;

•Studies and research for environmental protection and

territorial planning.

ENEA conducts scientific research and

technology development activities that draw on a

wide range of expertise, advanced facilities and

tools located at its own Research Centres,

operating in support of ENEA's programmes and

the Nation's productive system.

Photonics, nanotechnologies & nanophotonics

3

Photonics

is the science of the harnessing of light. Photonics encompasses the generation of light, the

detection of light, the management of light through guidance, manipulation, and amplification,

and most importantly, its utilisation for the benefit of mankind (Pierre Aigrain, 1967)

Nanotechnologies

technologies for realization and characterization of functionalized materials and devices with

enhanced properties based on the control of matter on a nanometric scale.

They include the ability to observe, measure and manipulate matter on an atomic and molecular

scale. In a simplified approach, “nano-products” are materials and/or devices with at least one

functional component sized less than 100 nm, but their relevance is related to nano-effects,

which lead to extraordinary enhancements in material properties.

Nanophotonics

science & engineering of light-matter interaction on a spatial scale comparable and/or less

than the wavelength of the e.m radiation, 300 nm at optical (UV-VIS-NIR) wavelenghts.

An International

Year of Light

and Light-based Technologies

2015

Luce ENEA C.R. Frascati

Imaging 15-16 ottobre, 2015

Microscopia:

Spettri di opportunita’

Point-light sources based on color

centers in LiF films for optical

imaging at high spatial esolution

Vertical planar microcavities

based on color centers in LiF films

for directional solid-state light-

emitting sourcesActive color center optical waveguides

in LiF crystals for miniaturised solid-state

lasers and amplifiers

Solid-state radiation

imaging detectors based on

LiF crystals and thin films

Broad-band organic light-emitting diode

(OLED) and thin films for displays, lasers and

photo-detectors

Xray microradiography of a

pollen (Olea europaea var.

ascolana) grains on a LiF

detector

CVD grown Si nanowires for nano-

electronics, photonics and sensors

Fiber Bragg Grating sensors in optical fibers and

technological applications

Si nanoparticles grown by laser

pyrolisis

Raman-SERS by nanostructured

metallic substrates

MNF – Photonics and nanotechnologies

Introduction and objectives

5

Since ancient times, X-ray and ion beams of different energies have been widely

investigated for many applications, including radiation diagnostics, radiobiology and

radiotherapy as far as medical applications are concerning.

Luminescent phenomena are successfully used in solid-state radiation detectors and

dosimeters based on point defects in insulating materials.

In the last decade, LiF crystals and polycrystalline thin films have been successfully tested

as novel solid-state detectors for X-ray imaging at nanoscale, based on the optical reading

of the photoluminescence (PL) of radiation-induced point defects emitting in the visible

spectral range.

On the other hand, doped (Mg, Ti, P) LiF materials are widely used in dosimetry

exploiting thermoluminescence (TL).

Very recently solid state LiF film radiation detectors, exploiting the PL of broad-band

light-emitting radiation-induced stable color centers (CCs), have been proposed and tested

for imaging and characterization of proton beams produced by a linear accelerator for

protontheraphy under development at ENEA C.R. Frascati, with the challenging aim of

investigate radiation dosimeters based on PL of CCs in this promising material.

Photoluminescence of radiation-induced CCs in LiF

6

LiF crystals and thin films can host laser active electronic defects, known as color centers

(CCs), characterized by wide tunability and high emission quantum efficiency, even at

room temperature (RT), utilized in solid state tuneable lasers and miniaturized light sources.

LiF crystals containing color centers induced

by gamma rays irradiation (Courtesy of Dr. V.

Kalinov, Minsk, Belarus).

Visible photoluminescence of LiF films

containing color centers, locally induced by

low energy electron beam irradiation, under

blue laser pumping.

R.M.Montereali, in Handbook of Thin Film Materials,

H.S.Nalwa ed., Vol.3: Ferroelectric and Dielectric Thin

Films, 2002, Academic Press, Ch.7, pp.399-431.

LiF and color centers

7

Nearest neighbour distance (Å) 2.013

Melting point (°C) 848.2

Density (g/cm3) 2.640

Molecular weight 25.939

Refractive index @ 640 nm, RT 1.3912

Solubility (g/100g H2O @ 25°C) 0.134

Hardness (Knoop 600 g indenter) 102

Transmission range (m) 0.12 - 7

Lithium Fluoride: alkali halide (AH) with fcc structure,

optically transparent from near UV to IR.

Among LiF peculiarities:

•it is almost non-hygroscopic;

• it can host CCs stable at RT;

•it can host laser active CCs tunable in a broad

wavelength range in the visible and near IR;

•polycrystalline LiF films can be grown by

thermal evaporation on different substrates.

Color Centers (CCs): point defects in insulating materials,

can be created in LiF by ionizing radiation,

like elementary particles and ions, as well as

photons, including soft and hard X-rays, rays and even

intense ultra-short (fs) laser pulses.

Irradiation of LiF gives rise to stable formation of primary and aggregate CCs, which

generally coexist with often overlapping absorption bands.

Optical properties of color centers in LiF

8

0.0

0.2

0.4

0.6

0.8

1.0

F2

-F

3

-F

3

+F

2

F2

-F

3

-

F3

+F

2

Absor

ption

400 600 800 1000 1200 14000.0

0.2

0.4

0.6

0.8

1.0

F2

+

F2

+

Wavelength (nm)

Emiss

ion

F2 and F3+ centers are laser active F-aggregate defects, consisting in two

electrons bound to two and three close anion vacancies, respectively.

F center is an anion vacancy occupied by

an electron; it is not active centers in LiF.

F2 ~ 18 ns; W32, W10 >> 1/

E3-E0 = 2.79 eV; E2-E1 = 1.83 eV

GS,

E0

URES, E3

W10

W32

1/

RES, E2

URGS, E1

Thermally evaporated polycrystalline LiF films

9

(a) (b)

(c) (d)

Ts

t

(a) (b)

(c) (d)

(a) t 1 m, Ts=30°C (b) t 1 m, Ts=300°C

(c) t 1.75 m, Ts=30°C (d) t 1.75 m, Ts=300°C on glass substrates.

oscillating quartzsubstrate

holder

crucible

Deposition parameters:

Pressure < 10-6 mbar

Evaporation rate

R = 0.5-2 nm/s

Film thickness t

up to 2 m

Substrate temperature

Ts=30-350°C

Nature of the substrateG.Baldacchini, M.Cremona, G.d'Auria, S.Martelli, R.M.Montereali,

M.Montecchi, E.Burattini, A.Grilli, A.Raco, NIM B 116(1996)447-451

LiF films of different thicknesses t grown at different substrate temperature Ts

LiF X-ray imaging detectors: principle of operation

10

substrate

LiF film

sample

CC layer

high densitylow density

X-rays

red and green

PL signal

substrate

LiF film

CC layer

high densitylow density

illuminating

blue light

Step 1:

Exposure/writing process

Step 2:

PL readout processReader:

photoluminescence

(PL) microscope

F2 and F3+ defects are

locally created in LiF by

X-rays.

Under blue light illumination,

the PL emission of F2 and F3+

defects locally created in the

areas previously exposed to

the X-ray beam, are observed.

The photoluminescent

patterns, stored in the

irradiated LiF detectors,

are acquired by using

optical microscopes in

fluorescence mode.

LiF radiation imaging detectors:

high spatial resolution on a wide field of view

11

2 mm 1) Conventional wide field fluorescence microscope

Soft X-ray micro-radiography of a dragonfly (Pyrrhesoma

nymphula) wing on a LiF film.

Near-field fluorescence optical microscope (SNOM)

30 x 40 um2 SNOM image of a mosquito wing micro-

radiograph stored in a LiF film

2) Confocal laser

fluorescence

microscope (CLSM)

Micro-radiography of a

mosquito (Diptera)

wing on a LiF film

50 nm spatial

resolution

250 nm

spatial

resolution

G.Baldacchini, F.Bonfigli, A.Faenov, F.Flora, R.M.Montereali, A.Pace,

T.Pikuz, L.Reale, J. Nanoscience and Nanotechnology 3,6(2003)483

A.Ustione, A.Cricenti, F.Bonfigli, F.Flora,

A.Lai, T.Marolo, R.M. Montereali, G.

Baldacchini, A. Faenov, T. Pikuz, L. Reale,

Appl. Phys. Lett. 88 (2006) 141107

12

F.Bonfigli, A.Faenov, F.Flora, M.Francucci, P.Gaudio, A.Lai,

S.Martellucci, R.M.Montereali, T.Pikuz, L.Reale, M.Richetta,

M.A.Vincenti and G.Baldacchini, Microscopy Research and

Techniques 71 (2008)35-41

Exudates are produced by Chlorella cells during their living conditions. Quantitative evaluations

of the signal along traces show less absorption ( in “negative” mode) with respect to the spherical

absorbing cells, which corresponds to the exudates.Biological sample: in vivo Chlorella sorokiniana Detector: LiF crystal (5x5x1)mm3, Protection layer

irradiated area: (250x250) m2

In vivo soft X-ray contact microscopy of Chlorella algae

X source: Nd:Yag laser plasma

source at University of Rome Tor

Vergata

N shot = 1, Target = Y,

Eww = 200 mJ/shot

E1keV = 100 mJ/shot

Solid-state radiation imaging luminescent LiF detectors

13

Peculiarities

Defect size 0.001 m

Readout: optical reading (PL)

Main characteristics

high spatial resolution ( intrinsic < 2 nm, standard 250 nm )

large field of view ( > 20 cm2, limited only by technologies of LiF film growth process)

efficiency of PL process (high emission quantum efficiencies of F2 and F3+ CCs in LiF)

stable storage of images (stability of CCs at RT in LiF)

Main advantages

•easy handling: no development need and no sensitivity to ambient light

•availability of readout instrumentation (PL excitation and emission in the visible range)G.Baldacchini, et al., Review Scientific Instruments 76(2005)113104-1,12 (Also selected for publication

in the Virtual Journal of Biological Physics Research 10(11), December 1, 2005) & Nanoforum 2011

• versatility: film geometry compatible with protective layers and different substrates

• multi-purpose: radiation sensitivity to X-ray (20 eV-40 keV), but also energetic photons

() and charged particles,

• wide dynamic range ( > 103), dependent on the used radiation, irradiation conditions, film

properties (and fluorescence reader characteristics)

In the last years, at ENEA C.R. Frascati, we propose^, realized and developed*

Novel soft X-ray imaging thin-film detectors based on photoluminescence (PL)

of radiation-induced ligth-emitting color centers in Lithium Fluoride (LiF)

^ENEA patent n. 514, N. TO2002A000575;

*ENEA patent n. 752, N. RM2012A000183

LiF film growth and confocal microscopy at ENEA C.R.

Frascati: Micro- and Nano-structures Laboratory

3 m thick LiF film on (5x5)

mm2 Si substrate produced by

ENEA Solid State Laser Lab

Commercial 0.5 m thick

PMMA film on (5x5) mm2

Si substrate

Nikon Eclipse

80i-C1 equipped

with an Argon

laser at 458 nm.

Proton irradiation facility

15

Proton beams were produced by a linear accelerator (LINAC) at ENEA C.R. Frascati.

TOP-IMPLART: Oncological Therapy with Protons – Intensity Modulated Proton Linear

Accelerator for RadioTherapy

SRIM software: The Stopping and Range of Ions in Matter, J.F. Ziegler,

M.D. Ziegler, J.P. Biersack; Nucl. Instrum. Methods B 268 (2010) 1818

2D LiF film radiation detectors for proton imaging

16

3 MeV proton beam image

on LiF film

Fluorescence Microscope: Nikon Eclipse 80-i,

s-CMOS camera: Andor NEO

Step 1:

Exposure of LiF sample to proton beams

Proton Beam parameters

•Energy: 3 MeV and 7 MeV (pulsed source @ 50 Hz)

•Actual Energy after 50 m thick kapton window:

2.23 MeV and 6.65 MeV

•Pulse duration: 60 ms Charge/pulse: 58 pC

•Beam diameter: ~ 3 mm

•Fluence range: 1011 – 1015 protons/cm2

•Proton implantation depth in LiF @ 2.23 MeV: 45 m

•Proton implantation depth in LiF @ 6.65 MeV: 295 m

M. Piccinini, F. Ambrosini, A. Ampollini, M.

Carpanese, L. Picardi, C. Ronsivalle, F. Bonfigli,

S. Libera, M.A. Vincenti and R.M. Montereali,

J. Lum. 156 (2014) 170-174

• Polished LiF crystals: 10x10 mm2, 1 mm thick

• Polycrystalline LiF films thermally evaporated

on glass substrates, 1 m thick

Step 2:

PL optical readout of CCs PL signal by

a conventional fluorescence microscope

Conclusions

17

•Novel two-dimensional (2D) LiF thin-film imaging detectors, sensitive to soft and hard X-

rays, utilising atomic-scale point defects as minimum luminescent units, are under

development.

•Soft X-ray micro-radiography and microscopy images have been already obtained with

sub-micrometric spatial resolution in LiF, even for in vivo cells.

•Solid-state LiF film luminescent radiation imaging detectors were successfully tested also

for hard X-rays from conventional X-ray tubes.

•The use of polycrystalline LiF thin films allows sub-micron spatial resolution even at

highest X-ray energies, suitable for radiation diagnostics.

•Accurate accumulated 2D dose distribution with high spatial resolution over large areas

were successfully demonstrated for the first time by using low energy proton beams.

• A wide dynamic range, covering three orders of magnitude of doses, together with non

destructive optical PL readout in a conventional optical microscope, was obtained in LiF thin-

films.

•Tissue equivalence of LiF materials makes their use attractive in radiation detectors based

on PL of CCs for clinical dosimetry, including hadrontheraphy, but

radiation sensitivity should be increased to measure low doses with great accuracy

Nanophotonics (control of light-matter interactions on a sub-micrometric scale)

& nanotechnologies (control of electronic defects at nanoscale)

Acknowledgements

18

Luce

Imaging

Microscopia:

Spettri di

Applicazione

ENEA

C.R. Frascati

15-16 ottobre,

2015

Acknowledgements

19

ENEA C.R. Frascati

UTAPRAD-SOR

F. Ambrosini,

A. Ampollini,

M. Carpanese,

L. Picardi,

C. Ronsivalle

S. Bollanti

P. Di Lazzaro

F. Flora

L. Mezi

D. Murra

UTAPRAD-DIM

Dr.ssa A. Lai

Dr. S. Almaviva

UTFUS

Dr. A. Rufoloni

Dip. Fisica Universita’Roma Tor Vergata

Dr. P. Del Gaudio

Prof. S. Martellucci

Dr.ssa M. Richetta

Integrated PL intensity vs fluence of 3 and 7 MeV

irradiated LiF crystals and thin films

20

• In LiF films the PL intensity is higher at the lower energy beam, because it is

proportional to the energy released into the film only 1m thick, at any fluence values.

• PL response of LiF films shows a linear behaviour covering several orders (2-3) of

magnitude of fluence range (estimated dose range 103-107 Gy)

In LiF crystals the PL

intensity is proportional to

the beam energy, which is

entirely released into the

crystal thickness, at any

fluence values, except at

saturation.

Increased collection efficiency: optical modelling

21

SPONTANEOUS EMISSION is

described by the interaction between

emitting dipole (CC) and

electromagnetic field distribution.

Introducing appropriate boundary

conditions it is possible to induce a

single CC to perform its optical cycle

faster, resulting in an increased time-

average photon emission amount.

Boundary conditions, such as mirrors in a planar microcavity, locally change the vacuum field,

which stimulates spontaneous emission and can increase the vertical confinement of emitted

green-red luminescence under blue optical excitation.E. Nichelatti and R.M. Montereali, J. Opt. Soc. Am. A 29, 3 (2012) 303-312.

0.1 0.2 0.3 0.4

30

210

60

240

90270

120

300

150

330

180

0

0.1 0.2 0.3 0.4

30

210

60

240

90270

120

300

150

330

180

0

Random dipole

emiss = 670 nm

pol. = S+PEnhancement: ~x 6

Exposure: laser plasma source at Rome

Tor Vergata University, Target Cu,

Single-shot, Distance source-LiF film:

4.5 cm, X-ray fluence ~350 mJ/cm2/shot

The photoluminescence signal

coming from the LiF film on Si

higher than the one collected from

the LiF film on glass and the ratio is

(1.76±0.11) , according with a fully

analytical model approach.

Increased radiation sensitivity of LiF film detectors

22

0 10 20 30 40 50 600

500

1000

1500

2000

2500

3000

3500

4000

4500

LiF film on silicon substrate

LiF film on glass substrate

gre

y le

vel

m

LiF film on glass LiF film on silicon

R. M. Montereali, F. Bonfigli, M.A. Vincenti and E. Nichelatti, Il

Nuovo Cimento 36 C, 2 (2013)

(b)

200 400 600 800 1000 1200 14000

20

40

60

80

100

R&

T (

%)

Wavelength (nm)

T

R

(a)

CLSM fluorescence images of X-ray contact micro-

radiographies of a nickel mesh (2000 lines/inch, 4 mm thick) on

LiF films (thickness ~ 1 m) irradiated in the same conditions.

Controlled manipulation of single atoms at AH surface

23

Ever since the 1990s, physicists have been able to directly control surface structures by

moving and positioning single atoms to certain atomic sites. A number of atomic

manipulations have previously been demonstrated both on conducting or semi-conducting

surfaces, mainly under very low temperatures. However, the fabrication of artificial

structures on an insulator at RT is still a long-standing challenge and previous attempts

were uncontrollable and did not deliver the desired results.

Using the tip of an atomic force microscope,

single bromine atoms were placed on a

sodium chloride (NaCl) surface to construct

the shape of the “Swiss cross”. The tiny cross

is made of 20 bromine atoms and was

created by exchanging chlorine with bromine

atoms. It measures only 5.6 nanometers

square and represents the largest number of

atomic manipulations ever achieved at RT.

It represents an important step towards the

fabrication of a new generation of

electromechanical systems, advanced

atomic-scale data storage devices and logic

circuits (S. Kawai et al, Nature

Commun.(2014)1-7)Source: http://www.unibas.ch/

Thank for your attention

24

Luce

Imaging

Microscopia:

Spettri di

opportunita’

ENEA

C.R. Frascati

8-9 ottobre,

2015

LiF film based radiation detectors : enhanced sensitivity

25

Crystal

The photoluminescence signal coming from the LiF film on Si is

significantly larger (8±2) than the one coming from the LiF

crystal:

light confinement effects in the investigated planar

microstructures (photonics)

polycrystalline films: high surface to volume ratio modifies

the CCs formation and stabilization processes (surface effects)

(R.M.Montereali, S.Almaviva, F.Bonfigli, A.Faenov, F.Flora, I.Franzini,

E.Nichelatti, T. Pikuz, M.A.Vincenti, G.Baldacchini, Proc. SPIE Vol.

6593, 2007).

LiF crystalAFM image of the surface of a LiF

film 3.3 m thick thermally

evaporated on a glass substrate at Ts

= 280°C.LiF film on Si

The reflective properties

of Si help to recover a

relevant part of lost PL.

Radiation diagnostics: soft X-ray scientific imaging

26

X-ray imaging at the nano- and micro-scale is of great interest, also for biological samples.

Optical Microscopy (OM)

Abbe diffraction limited, ~300 nm for visible light;

novel super-resolution fluorescence technique to

detect the marked fluorescent molecules.

Electronic Microscopy (SEM e TEM)

Limited by preliminary treatments of

sample (dehydration, fixing and dying

with electron dense substances).

Soft X-Ray Microscopy

( : 10 - 0.1 nm , E: 200 eV – 5 keV)

internal structure of samples at a high spatial resolution and

avoiding all specimen preparation

(biological samples also in their normal living state).

The short wavelength gives the potential for high-resolution

imaging.X-ray

microscope

image of the

labelled

microtubule

network in a

whole, hydrated

mammary

epithelial cell.

Photo courtesy

of C. Larabell

X-ray

radiography of

the hand of

Röntgen’s wife

(1896)

Micro-radiography of a dragonfly (Pyrrhesoma

nymphula) wing

27

2 mm

Plasma

10 cm L i F f i l m

X e C l L a s e r :

1 J - 1 0 n s

C u t a p e

t a r g e t

b i o l o g i c a l s a m p l e

X - r a y s

C o l o r

c e n t e r s

g e n e r a t i o n

Biological sample: dragonfly (Pyrrhesoma nymphula) wing

Detector: 2 m thick LiF film evaporated on glass,

Exposure: LPP at ENEA C.R. Frascati,

Rotating metallic target: copper, tantalum, iron, etc,

= 60 – 0.6 nm, h = 2 keV - 20 eV, Emax = 250 eV

Sample-Source distance: 5 – 15 cm on the normal

Tight laser focusing, point-like source behaviour

Radiation dose uniform on a large area, up to

(4x4)cm2, W ~ 0.15 mJ/cm2/shot, P~3GW/cm3/shot

G.Baldacchini, F.Bonfigli, A.Faenov, F.Flora, R.M.Montereali, A.Pace,

T.Pikuz, L.Reale, J. Nanoscience and Nanotechnology 3,6(2003)483

Wing micro-radiography on a 2 m thick LiF film at optical microscope obtained by observing

the photoluminescence (PL), under the laser pumping wavelength of 458 nm.

Optical readout: fluorescence microscopy

28

500 550 600 650 700 750 8000

20

40

60

80

100

red filter

green filter

F2 and F

3

+ PL spectra

F3

+

F2

ph

oto

lum

ine

scen

ce

(a

rb. u

n.)

CL

SM

filte

r tr

an

sm

itio

n %

(nm)

The CLSM system allows the specimen to be sectioned

optically by scanning a series of plane eliminating

interference from adjacent, overlying and underlying

fluorescence.

Only in focus ligth arrives at the detector; all out-of-

focus ligth is eliminated.

The confocal system allows to reach a higher lateral

resolution respect to conventional fluorescence

microscopes (resolution is increased up to 30% respect

to conventional wide-field microscopes).

The ENEA system is a Nikon Eclipse 80i

equipped with an Argon laser at 458 nm. SNOM collection mode - (CNR-ISM)

F2

F3+

29

Water Window

4.4 - 2.3 nm (0.28 - 0.53 keV)

Carbon Window

5 - 4.4 nm (0.25 - 0.28 keV)

Oxygen K edge

Soft X-ray

1-4 nm (1000 – 300 eV)

EUV

4 – 60 nm (300 – 20 eV)

Carbon K edge

For the soft X-ray microscopy,

the 2.3-4.4 nm wavelength

interval (called water-window,

ww) is usually used, because of

the strong absorption of carbon

(as compared with that of

water) which allows to obtain a

natural contrast in cells

imaging. The spectral range,

which immediately follows the

carbon K-edge on the long-

wavelength side (carbon

window) is characterized by a

largest radiation penetration

depth into carbon compounds

and the differences in the

absorption coefficients of

cellular structures and other

substances is 5-6 times larger

than in the ww.

The water and the carbon windows

Soft X-rays irradiation of LiF

30

*ENEA patent n° TO2002A000575,

N. WO2004/005906 A1 del 15/01/2004.

0 200 400 600 800 1000 1200 1400 1600 1800 20000

1

2

3

4

5

6

Photon energy ( eV)

Att

enu

ati

on

len

gth

in

LiF

(m

)

EUV SXR

SXR: 0.3 < h < 3 keV

WW : 4.4 - 2.3 nm (0.28 - 0.53 keV)

- See smaller features* X-ray microscopy

- Write smaller patterns* EUV Lithography

100 1000 100000.01

0.1

1

10

100

1000

10000

Att

en l

ength

(

m)

Photon Energy (eV)

Atten length

(CuKa, LiF) ~ 330 m

8.042 keV,

Cu-K

X-ray tubes

13.5 nm, ~90 eV, EUVL

Low scattering cross-section:

it limits lateral spreading of the beam.

Neutrality: it avoids surface charge effects in

insulating materials.

Low penetration depth, dependent from the

selected energy.

0 20 40 60 80 100 1200

20

40

60

80

100

Photon energy ( eV)

Att

enu

ati

on

len

gth

(n

m)

Luminescent radiation detectors based on doped LiF

31

Thermoluminescence Dosimeter

(TLD) glow curve

Doped LiF pellets, powders, …

TLD100

LiF:Mg:Ti 420-460 nm

GR200 TLDHS

LiF:Mg:Cu:P ~ 380 nm

Luminescent phenomena are successfully used in solid-state radiation detectors and

dosimeters based on point defects in insulating materials. Among them,

thermoluminescence (TL) in doped LiF , an alkali halide, radiation sensitive material.

Comparison with similar detectors for X-ray imaging

32

Photographic film (Kodak DEF)

Grain size 1.5 m

Fluence dynamic range: 1 nJ/cm2 – 0.1 mJ/cm2

Readout: development + optical reading (absorption)

Drawback: no visible light exposure

Photoresist PMMA

Molecule size 0.01 m

Fluence dynamic range: (1 – 50) mJ/cm2

Readout: development + AFM

LiF luminescent detector

Defect size 0.001 m

Fluence dynamic range: 0.1 mJ/cm2 – 1 J/cm2

(under investigation)

Readout: optical reading (PL)

high spatial resolution

wide dynamic range

large field of view

stable storage of images

simplicity and efficiency of readout process

easiness of use & versatility

no need development

Image Plate, IPs (Fuji HR-S)

Grain size 5 m

Fluence dynamic range: 1 pJ/cm2 – 0.1 mJ/cm2, linear

Readout: optical reading (OSL)

Drawback: fading

LiF X-ray imaging detectors: principle of operation

33

Irradiated

LiF detector

Pumping ligth (458-488 nm)

300 400 500 6000.0

0.2

0.4

0.6

0.8

1.0

Ab

s (

norm

.)

wavelength (nm)

F2

F3

+

Photoluminescence of

F2, F3+ CCs (535-670 nm)

400 600 800 1000 12000.0

0.2

0.4

0.6

0.8

1.0

OS

L (

norm

.)

wavelength (nm)

F2

F3

+

X-RAY

LiF detector

Irradiated

LiF detector

Permanent fluorescent patterns based

on F2 and F3+ defects in LiF can be

produced by using several X-ray sources

in different configurations (contact mode,

direct writing, projection mode, etc.)

The photoluminescent patterns, stored in the

irradiated LiF detectors, are observed by using

optical microscopes in fluorescence mode.

Illumination with blue light excites the visible

photoluminescence of the F2 and F3+ defects locally

created in the areas previously exposed to the X-ray

beam.

Exposure/writing process Readout process: photoluminescence (PL) microscopy

Permanent fluorescent patterns based

on F2 and F3+ defects in LiF can be

produced by using several X-ray sources

in different configurations (contact mode,

direct writing, projection mode, etc.)

Formation and stabilization of CCs: surface effects

34

The irradiation of alkali halide with ionizing radiation starts processes of defect creation and

diffusion which strongly affect the crystal surface. On the other hand, surface effects in

polycrystalline HA affects the formation and stabilization of color centers.

•The atomic coordination at the surface is not fully comparable to the atoms within a crystal.

•The surface atoms have neighbors on only one side, therefore they are less firmly bonded

than the internal atoms.

•They have broken bonds which make them more reactive.

•Mismatch between grains results in edge dislocations at the interface.

•Large disorder at the grain boundaries result in large gaps in the material.

However the possibilities for surface investigations of alkali halides, are quite restricted

because most of the standard surface-sensitive techniques, especially electron spectroscopies,

are difficult to use.

Edge dislocationsGrain boundaries